Optics and Laser Technology 118 (2019) 93–101

Contents lists available at ScienceDirect

Optics and Laser Technology

journal homepage: www.elsevier.com/locate/optlastec

Full length article

Mode-locked pulse generation in erbium-doped fiber laser by evanescent T

field interaction with reduced graphene oxide-titanium dioxide nanohybrid
⁎
H. Ahmad , S.A. Reduan, N. Yusoff, M.F. Ismail, S.N. Aidit
Photonics Research Center, University of Malaya, 50603 Kuala Lumpur, Malaysia

H I GH L IG H T S

• rGO-TiO nanohybrid prepared by the hydrothermal method.

2

• The D-shape fiber is covered with rGO-TiO nanohybrids as a saturable absorber.

2

• Passive soliton mode-locking operations is experimentally demonstrated.

• The pulse width of 1.05 ps is obtained at repetition rate of 11.19 MHz.
• Lasing with centre wavelength of 1560.45 nm and 3–dB bandwidth of 2.47 nm.

A R T I C LE I N FO A B S T R A C T

Keywords: In this work, a new nanohybrid saturable absorber (SA) is successfully fabricated from reduced graphene oxide
Fiber laser (rGO) nanosheets and titanium dioxide (TiO2) nanoparticles. The nanohybrid material is synthesized using the
Mode-locked simple and inexpensive hydrothermal technique. The SA is fabricated by depositing the nanohybrid solution
Nanohybrid onto a D-shaped fiber in an erbium-doped fiber (EDF) laser cavity. The evanescent wave interaction between the
Reduced graphene oxide
incident light and rGO-TiO2 nanohybrid material induces mode-locking in the EDF laser at the threshold pump
Titanium dioxide
power of 100.80 mW. A stable soliton pulse with a center wavelength of 1560.45 nm and 3-dB bandwidth of
2.47 nm is obtained. The generated pulses have a repetition rate and pulse width of 11.19 MHz and 1.05 ps at the
highest pump power of 268.10 mW. The proposed rGO-TiO2 nanohybrid of this work is a promising SA material
for generating mode-locking in an EDF laser for optical modulation applications.

1. Introduction induce modulation on the electromagnetic field of the signal propa-

Fiber lasers capable of generating ultrashort output pulses have
attracted the attention of researchers around the world due to their
significant advantages that include excellent heat dissipation and
freedom from alignment. These lasers also have a compact cavity design
as well as the ability to generate high quality pulses in the picosecond
and subpicosecond durations with a wide tunable wavelength span
covering several tens of nanometers [1–3]. As a result of these abilities,
ultrashort pulse fiber lasers have high potential to be used as sources in
various applications such as biomedical diagnostics, optical fiber
communications, supercontinuum generation and material processing
[4–6].
In general, ultrashort optical pulses can be generated through either
active or passive mode-locking techniques. Active mode-locking is ob-
tained using an external signal, such as an acousto-optic modulator to
gating within the laser cavity [7]. Passive mode-locking operation on
the other hand is initiated by a non-linear element such as a bleached
saturable absorber (SA) which has negligible loss when high intensity
excitation is applied [8]. Of the two, passive methods are typically the
preferred method of inducing mode-locking, due to its compact size,
simplicity and flexibility as not requiring external synchronized driving
circuits [9].
In the past few years, there has been extensive focus on the devel-
opment of passively mode-locked fiber lasers using SAs based on low
dimensional materials such as carbon nanotubes [10,11], graphene
[8,12–14], black phosphorus [15,16], transition-metal dichalcogenides
(TMDs) [17–20], and topological insulators (TIs) [21–23]. These ma-
terials exhibit strong optical saturable absorption [24], and have a
scalable bandgap which allows the operating wavelength band and
modulation depth to be adjusted [16]. As a result of its broadband

⁎
Corresponding author.
E-mail address: harith@um.edu.my (H. Ahmad).

https://doi.org/10.1016/j.optlastec.2019.05.015
Received 28 December 2018; Received in revised form 18 April 2019; Accepted 7 May 2019
0030-3992/ © 2019 Published by Elsevier Ltd.
H. Ahmad, et al.
Fig. 1. (a) Schematic diagram of the rGO-TiO2 nanohybrid deposited on the D-shape fiber and (b) its corresponding optical microscopy images. (c) Cross-section of
the D-shape fiber.
saturable absorption, ultrafast recovery time, controllable modulation
depth and easy fabrication, graphene has long been seen as the most
versatile and attractive SA material for the design of mode-locked fiber
lasers [25]. This has been proven with a passively mode-locked fiber
laser generating a 670 fs pulse with a spectral width of 4.99 nm at a
central wavelength of 1557.14 nm by the incorporation of a graphene
thin film SA by Lau et al. [8]. Additionally, Bao et al. [26] demonstrated
the formation of short laser pulse using graphene as an SA in which the
output pulses exhibited a center wavelength, spectral width, and re-
petition rate of 1561.6 nm, 1.96 nm, and 6.99 MHz respectively.
In spite of its remarkable advantages, graphene still suffers from a
number of inherent weaknesses such as a weak absorption coefficient of
only 2.3% of incident light per layer, zero bandgap, and susceptibility
to damage at even medium intracavity laser intensities. In order to
overcome these drawbacks, graphene has now been hybridized with
metal oxide nanoparticles to form a new binary composite material that
combines the excellent optical properties of graphene and the strong
mechanical qualities of the metal oxide. Among the metal oxides, ti-
tanium dioxide (TiO2) is intensively investigated as it has desirable
characteristics such as higher optical nonlinearities, wide indirect
bandgap, high transmittance in the visible region and a high refractive
index [27]. Therefore, the combination of graphene nanosheets with
TiO2 nanoparticles is expected to exhibit exceptional properties with
complementary performance and multi-functionalities for various ap-
plications.
In this work, a passively mode-locked EDF laser using rGO-TiO2
nanohybrid particles are deposited onto a D-shaped optical fiber as an
SA to induce mode locking in an erbium doped fiber laser (EDFL)
cavity. The rGO-TiO2 nanohybrid is first synthesized via a hydrothermal
process with titanium isopropoxide (TiIP) and graphene oxide (GO) as
precursors for TiO2 and rGO, respectively. The D-shaped optical fiber is
manually fabricated from a single mode fiber (SMF-28) using a pol-
ishing film, and the nanohybrid materials are then deposited onto its
polished surface. Upon the integration of the SA into the laser cavity,
stable soliton pulses with significant Kelly sidebands are achieved at a
pump power of 100.8 mW from the interaction of the evanescent field
94
Optics and Laser Technology 118 (2019) 93–101
of the incident light and the rGO-TiO2 nanohybrid material layer. The
use of the D-shaped optical fiber allows for guided waves to propagate
in the waveguide unhindered while still interacting significantly with
the nanohybrid SA material. Therefore, a low mode locking threshold
and high output power can be achieved in an all-fiber configuration
[28]. The results obtained in this work indicate that the rGO-TiO2 hy-
brid material has remarkable potential as an SA for ultrafast pulse
generation in various photonics applications. To the best of the author’s
knowledge, this is a first demonstration of rGO-TiO2 nanohybrid par-
ticles deposited on a D-shaped optical fiber as an SA in a passively
mode-locked EDFL.
2. Preparation and characterization of rGO-TiO2
The rGO-TiO2 nanohybrid is prepared using the hydrothermal
method. In the first step, 1 M of an ionic titanium (IV) (Ti4+) solution is
prepared by mixing TiIP with triethanolamine (TEA). The solution is
stirred for 30 min under ambient conditions and an appropriate amount
of the Ti4+ ionic solution is then added dropwise into a 25 mL graphene
oxide (GO) solution at 10 mg•mL−1 while being stirred. The GO solu-
tion is prepared by the oxidation of graphite flakes using a simplified
Hummers’ method [24]. The mixture is stirred continuously at room
temperature until a homogenous suspension is obtained and is then
transferred to a Teflon lined autoclave before being placed in an oven
and treated for 24 h at 180 °C. After the hydrothermal treatment, the
autoclave is cooled to room temperature before the washing process
continues. The black precipitate obtained is washed several times with
deionized (DI) water and ethanol before being put into a centrifugre at
4000 rpm for 30 min, forming a black slurry which is dried in an oven
for overnight at of 60 °C. This final product obtained is the desired rGO-
TiO2 nanoparticle powder.
The fabrication process for the D-shape fiber covered with the rGO-
TiO2 nanohybrid material is given in Fig. 1. In the first step, the D-
shaped optical fiber is fabricated by polishing one side of a standard
SMF-28 that has been clamped to the polishing rig by fiber holders. The
D-shaped fiber is then transferred to a clean glass slide with the
H. Ahmad, et al. Optics and Laser Technology 118 (2019) 93–101

rGO-TiO 2 254 rGO-TiO2 (c) 1355 rGO-TiO2

(a)
(b) 1597
I D/IG = 0.99

TiO2

(154)
417
(1 0 1)

TiO2

Absorbance (a.u.)
Intensity (a.u.)

Intensity (counts)
TiO2

(644)
(516)
(405)
(2 0 0)
(0 0 4)

(1 0 5)
(2 1 1)

(2 0 4)

(2 1 5)
(1 1 6)
(2 2 0)
rGO

rGO 415
rGO
ID/IG= 1.04

GO

I D/IG= 0.88
20 30 40 50 60 70 80
2θ ( °) 300 400 500 600 700 500 1000 1500 2000 2500
Wavelength (nm) Raman Shift (cm-1)

Fig. 2. Characterization of rGO-TiO2 nanohybrid: (a) XRD diffraction pattern, (b) UV–vis spectrum, (c) Raman spectrum (Insert: Raman spectrum for graphene oxide
(GO)), and (d) FESEM image.

Table 1
Saturable absorption measurements of rGO, TiO2 and rGO/TiO2 material
based–SA.
Material Modulation Depth (%) Saturation Intensity (kW/cm2)

rGO ∼49 0.2

TiO2 ∼54 0.25
rGO-TiO2 ∼32.54 0.42

Table 2
Measured PDL values side-polished fibers with of rGO, TiO2 and rGO-TiO2
material based-SA.
rGO-TiO2 rGO TiO2

Polarization Dependent Loss (dB) 0.38 1.6 0.3

polished face facing upwards before approximately 5 µL of the rGO-

Fig. 3. Non-linear absorption spectra of the prepared rGO-TiO2 coated D-shape TiO2 nanohybrid solution is slowly dropped onto the polished surface
fiber SA. using a micropipette. No additional polymers are used to coat the top of
the deposited rGO-TiO2 layer. The insertion loss of the D-shaped fiber is
measured to be 2.98 dB and increases to 5.72 dB after the deposition of
the nanohybrid material onto the polished surface. The polishing length

95
H. Ahmad, et al. Optics and Laser Technology 118 (2019) 93–101

and core-cladding distance are measured to be 369.97 μm and

11.09 μm, respectively, with the rGO/TiO2 interaction length estimated
to be ¾ of the polishing length.
The crystalline structure and composition of the rGO-TiO2 nano-
hybrid is analyzed using an Empyrean PANalytical X-ray diffractometer
(XRD) with monochromatized copper (Cu) Kα radiation at an excitation
wavelength, λ = 1.5418 Å. The system is operated at a scanning rate of
0.02° per second over a 2θ range of 20° – 80°. Fig. 2(a) shows the XRD
pattern obtained from the rGO, TiO2, and rGO-TiO2 nanohybrid in its
powder form. Based on the XRD pattern of TiO2, the diffraction peaks at
2θ = 25.3, 37.9, 47.8, 53.8, 54.8, 62.6, 68.5, 69.9, and 74.8° corre-
spond to the (1 0 1), (0 0 4), (2 0 0), (1 0 5), (2 1 1), (2 0 4), (1 1 6),
(2 2 0), and (2 1 5) planes of TiO2. This XRD pattern is consistent with
the standard XRD data for tetragonal phase anatase TiO2 in accordance
to the JCPDS card no. 21-1272 [29]. Two broad but weak peaks at
∼27° and ∼42° are observed in the XRD pattern of the rGO sample,
which can be assigned to the (0 0 2) and (0 0 1) peaks respectively of
exfoliated graphene [30]. The diffraction patterns observed for the rGO-
TiO2 nanohybrid sample match well with standard TiO2 patterns, with
Fig. 4. The schematic diagram of the passively mode-locked EDF laser with the
the existence of strong and sharp diffraction peaks demonstrating that
rGO-TiO2 coated D-shape fiber SA.
the TiO2 nanoparticles possess good crystallinity with high purity. This
is confirmed from the fact that no other diffraction peaks are observed.
Table 3 In addition to that, the characteristic peak of graphene which normally
Numerical estimation of GVD of fibers used in proposed experiment. appears at 2θ = ∼27° overlaps with the diffraction of the dominant
Type of fiber Fiber length (m) λ (nm) D (ps/nm/km) GVD (ps2/km) (1 0 1) plane of TiO2 [31]. Furthermore, the complete coverage of TiO2
on the rGO sheets also results the no obvious diffraction peaks for rGO.
SMF-28 17.95 1560 18 −23.3 This result reveals the presence of a crystal structure in the anatase
EDF 0.5 −18 +23.3
phase TiO2 particles of the nanohybrid and confirms the formation of

Fig. 5. Output characteristics of mode-locked fiber laser coupled with D-shape fiber coated with rGO-TiO2 nanohybrid as SA: (a) the output optical spectrum, (b)
pulse train, (c) output autocorrelation trace, and (d) RF spectrum. Inset: The broadband frequency spectrum from 10 to 110 MHz.

96
H. Ahmad, et al. Optics and Laser Technology 118 (2019) 93–101

Table 4 to the D and G bands respectively [36]. The D peak relates to the defects
The comparison of the mode-locked pulsed laser parameters for rGO, TiO2 and and disorder that activates the Raman mode due to the vibrations of the
rGO-TiO2 material based-SA. sp3 carbon atoms, while the G peak originates from sp2 hybridized
rGO-TiO2 rGO TiO2 carbon atoms in 2D hexagonal graphitic [32]. The D to G band intensity
ratio (ID/IG) of rGO is measured to be 1.04, which is larger than the ID/
Center wavelength (nm) 1557.80 1558.40 1560.45 IG ratio for GO of 0.88, due to the introduction of a significant number
Pulse duration (ps) ∼0.76 ∼0.80 1.05
of structural defects to the graphene lattice after the reduction process.
Repetition rate (MHz) 16.3 16.1 11.18
Pump power range (mW) 205.40–280.50 252.10–280.50 100.80–280.50 This also indicates the successful removal of oxygen functionalities
Output Power (mW) 1.94 2.07 1.43 from the surface of GO, thus proving the successful reduction of GO into
Pulse Energy (pJ) 119.02 128.57 127.96 rGO upon the hydrothermal reaction. Interestingly, the ID/IG ratio for
rGO-TiO2 nanohybrid decreases slightly to 0.99 which suggests that
TiO2 nanoparticles had occupied most of the vacancies in rGO, thereby
recovering the defects. In addition, three characteristic Raman-active
modes are observed at 154, 405, and 644 cm−1 which are assigned as
the Eg, B1g, and Eg band of the anatase TiO2 phase [37]. The presence of
characteristics Raman modes for TiO2 and rGO has become the evi-
dence for the successful formation of the rGO-TiO2 nanohybrid.
The morphology and structure of the rGO-TiO2 nanohybrid is stu-
died using a Hitachi SU8220 field emission scanning electron micro-
scope (FESEM) operating at 2.0 kV. Fig. 2(d) provides the obtained
FESEM image of the synthesized rGO-TiO2 nanohybrid. As can be seen
from the image, the presence of TiO2 nanoparticles exhibit an irregular
spherical shape with an average diameter size of ∼11.50 nm. The TiO2
nanoparticles are observed to be tightly anchored and evenly dis-
tributed on the surface of rGO sheets due to the presence of large
number of polar groups in the GO precursor which served as an anchor
that provides more nucleation sites for the formation of TiO2 nano-
particles. This result further confirms the successful preparation of the
rGO-TiO2 nanoparticles via the hydrothermal treatment.
In order to determine the modulation depth of the rGO-TiO2 SA, a
twin detector method is conducted by using a homemade mode-locked
EDF laser incorporation with carbon nanotubes (CNT) SA as the pulse
seed. The pulse seed which acts as the laser source possesses a pulse
width of 1.12 ps, repetition rate of 27.78 MHz, and output power of
4.68 mW at a central wavelength of 1566.4 nm. A variable optical at-
tenuator is used to control the input power to the fabricated SA. The
variation of the optical absorbance of SA with respect to different input
intensities is recorded and the nonlinear saturable absorption curve of
Fig. 6. Variation of the pulse shapes of the output laser with different pump the rGO-TiO2 coated D-shape fiber SA is depicted in Fig. 3. The non-
powers. linear parameters are obtained by fitting the measured data to a theo-
retical model as expressed below [38]:
the rGO-TiO2 nanohybrid. αs
α (I ) = + αns
A Varian Cary 50 UV–visible spectrophotometer is used to measure 1 + I / Isat
the UV–vis absorption spectrum of rGO-TiO2 nanohybrid in its solution
form. The UV–visible absorption spectra of the rGO, TiO2, and rGO- where α(I) is absorption, I is input intensity, αs is saturable absorption
TiO2 nanohybrid nanoparticles are recorded in the range of or modulation depth, αns is non-saturable absorption and Isat is sa-
200–700 nm and given in Fig. 2 (b). The UV–vis absorption spectrum of turation intensity. From the fitted graph of the nonlinear absorption
rGO shows an absorption peak at 254 nm which is attributed to the curve as a function of pump power intensity, the modulation depth of
effective restoration of the sp2 carbon networks (C]C bonds) within rGO-TiO2 is evaluated to be 32.54% with a saturation intensity and
the rGO sheets after reduction [32]. Meanwhile, the TiO2 sample ex- non-saturable loss of about 0.42 kW•cm−2 and 67.46%, respectively.
hibits an absorption edge threshold at 415 nm which is in agreement The saturable absorption parameters of the rGO, TiO2 and rGO-TiO2
with the previous report [33]. As can be seen from the UV–vis spectrum nanoparticles are shown in the Table 1. From the table, it can be seen
of the rGO-TiO2 nanohybrid, a broad peak appears at 254 nm which is that TiO2 has a higher modulation depth as compared to rGO and the
in accordance to the characteristic absorption peak of rGO [34]. An- hybrid rGO-TiO2, while rGO has the lowest saturation intensity as
other absorption peak at 417 nm could also be observed, corresponding compared to the other two materials. The hybrid rGO-TiO2 has the
to the absorption of TiO2 [35]. This further validates that TiO2 nano- lowest modulation depth and higher saturation intensity as compared
particles have grown on the surface of the rGO nanosheets after the to rGO and TiO2. As observed by J. Jeon et al. [39], zero cavity GVD
hydrothermal process. needs a much higher modulation depth to generate a stable pulsed
Further characterization of the rGO-TiO2 nanohybrid is carried out laser. Since this work has a GVD of −0.405 ps2, the nanohybrid ma-
by micro-Raman measurements using a Renishaw Raman Microscope terial is a suitable material to be used in the cavity, with the modulation
with an argon ion laser at 514 nm at room temperature as the excitation depth of 32.54% comparable to previous works by Hu et. al. [40]. Thus,
source. Fig. 2 (c) shows the Raman spectra of GO, rGO, TiO2, and rGO- the combination of TiO2 with rGO results a suitable saturable absorber
TiO2 nanohybrid recorded from 200 to 2500 cm−1. Two prominent to be used in this work in terms of its nonlinearity characteristics. The
peaks could be observed in the Raman spectrum of GO and rGO which saturation intensities for all these materials are lower than commonly
is associated with the characteristic peaks of graphene that correspond reported by previous works, and could be advantageous in generating a
pulsed laser output [41].

97
H. Ahmad, et al.
Fig. 7. (a) 3D plot of RF spectra measured under different time, and (b) output stability measurement of the prepared laser over 60 min observation period.
The PDL values for the D-shaped fibers with rGO, TiO2 and rGO-
TiO2 deposited onto its polsihed surface is given in Table 2.These re-
sults confirm that a PDL of 0.38 dB is not high enough to induce non-
linear polarization rotation to generate mode-locked lasing in the EDFL
cavity, as a much higher PDL is necessary to induce mode-locking by
NPR [42]. Even though the PDL of rGO is highest among other two
materials, it is still not adequate enough to generate mode-locking by
NPR. As such, it can be concluded that the nanohybrid material de-
posited on D-shaped fiber is the exclusive factor in generating the
mode-locked output from the EDFL.
3. Experimental setup
The passively mode-locked EDFL configuration is given in Fig. 4.
A 974 nm laser diode (LD) is used to drive a 50 cm long erbium-
98
Optics and Laser Technology 118 (2019) 93–101
doped fiber (EDF) with an absorption coefficient of 250 dB/m at
980 nm and 16 dB/m at 1530 nm. A 980/1550 nm wavelength division
multiplexer (WDM) is used to connect the LD to the EDF, with the LD
being connected to the 980 nm port of the WDM and the EDF being
connected to the WDM’s common port. The output from the EDF is
connected to a polarization insensitive isolator (PI-ISO) and subse-
quently the rGO-TiO2 side-polished D-shape fiber. A polarization con-
troller (PC) is connected to the output of the SA, and is in turn con-
nected to a 90/10 output coupler, whose 90% port is connected to the
1550 nm port of the WDM and thus completes the optical circuit. The
PI-ISO is used to ensure the unidirectional operation of the ring cavity,
while the 10% port of the coupler is used to extract a portion of the
signal for analysis. The PC is used to alter the intra-cavity birefringence
of the laser resonator as well as optimizing the fiber laser performance.
The total cavity length is estimated to be around 18.45 m, consisting
H. Ahmad, et al. Optics and Laser Technology 118 (2019) 93–101

of the enhanced resonance effect between solitons and their respective

shedding wave radiated by the pulse, which are periodically perturbed
by the gain stimulated by the EDF and lost from the laser output
[43,44]. The results suggest that the passively mode-locking operation
works in the anomalous dispersion regime [45].
The output mode-locked pulse train corresponding to a repetition
rate of 11.19 MHz is presented in Fig. 5(b), which is in good agreement
with laser cavity length of 18.45 m. The pulse trace shows a relatively
uniform intensity with the interval between adjacent pulses measured
to be about 89.40 ns. This result is consistent with the optical cavity
round trip time of 89.37 ns. Fig. 5(c) depicts the measured auto-
correlation trace of the output pulse which can be well fitted to a secant
hyperbolic (Sech2) temporal profile. The full width at half maximum
(FWHM) of the pulse duration is measured to be 1.05 ps, giving a time
bandwidth product (TBP) of 0.319.
The result demonstrates that the output pulses are slightly chirped
as the calculated TBP value is slightly higher than the Sech2 transform-
limited TBP value of 0.315. This is due to the chromatic dispersion in
relatively long fiber pigtails at the laser output that results in slight
deviation of the TBP value [46]. The radio frequency (RF) spectrum at
Fig. 8. Output power and pulse energy versus pump power. the fundamental repetition rate, fo of 11.19 MHz with 300 Hz resolution
bandwidth (RBW) is illustrated in Fig. 5(d). The electrical signal-to-
Table 5 noise ratio (SNR) of the output pulse is measured to be about 62.90 dB,
Comparison of the parameters observed in this work against others D-shape indicating highly stable mode-locking. Based on the RF spectrum re-
fiber based mode-locked lasers using different SAs. corded at broader frequency span of up to 110 MHz, as given in the
inset of Fig. 5(d), the harmonic frequency components are present. This
Type of SA Graphene MoS2 GO Graphite rGO-TiO2
further confirms the high stability of the generated mode-locked pulses
Operation 1561.6 1565.39 1555.7 1567 1560.45 in the proposed laser cavity.
wavelength Table 4 simplifies the output performance of the rGO, TiO2, and
(nm) rGO-TiO2 at a pump power of 268.10 mW. From the table, the rGO-TiO2
Max. pulse energy 7.25 nJ – – 83 pJ 134.98 pJ
Repetition rate 6.99 MHz 4.17 MHz 16.5 MHz 15.7 MHz 11.19 MHz
based-SA generates a mode-locked pulsed laser at longer wavelength as
Pulse duration 1.3 ps 116 ps 1.18 ps 220 fs 1.05 ps compared to SAs based on their individual materials. However, while
Ref. [26] [51] [52] [53] This work the nanohybrid material has a longer pulse duration and smaller re-
petition rate, it has a lower threshold pump power as shown in the
table. Although the output power of nanohybrid is lower than the
of 17.95 m of single-mode (SMF-28) fibers and 0.5 m of EDF. This gives output power of pulse laser by TiO2, the pulses energy is comparable.
an estimated group velocity dispersion (GVD) of –23.3 ps2/km and This shows that the nanohybrid material can generate mode-locked
+23.2 ps2/km respectively at 1560 nm, as stated in Table 3. From output pulses at the lower pump power and longer center wavelength.
Table 3, the total cavity dispersion is −0.405 ps2, which indicates that It is suggested that the charge transfer between TiO2 and rGO con-
the laser will operate in the anomalous dispersion region and is thus a tributed in the improvement of the SA performance [47]. A large
soliton fiber laser. transient populations of carriers in the conduction band (CB) and va-
The output characteristics of the pulse emissions are recorded by an lence band (VB) are produced upon the laser irradiation on the nano-
Anritsu MS9740A optical spectrum analyzer (OSA) with a scanning hybrid material due to the zero bandgap of rGO. The excited electrons
range of 0.6–1.75 µm and a resolution of 0.03 nm for spectral analysis, in the CB of rGO has higher probability of transferring to the metal than
while a 2.5GS/s-500 MHz bandwidth Yokogawa DLM2054 mixed signal to the VB of rGO on account of the larger density of states in the TiO2.
oscilloscope (OSC) coupled with a 1.2 GHz photodetector is used to The bleaching of the ground state started to takes place attributed to the
analyse the spectral and output pulse train characteristics of the in- fast excitation of the carriers compared to their relaxation from the
duced pulses. An Anritsu MS2683a radio-frequency spectrum analyser metal state to the VB of rGO. Therefore, a stronger SA effect occurs at
(RFSA) and an Alnair Labs HAC-200 optical intensity autocorrelator are the lower thershold pump power, making the rGO-TiO2 nanohybrid as
also used to characterize the outputs of the cavity. excellent candidate as SA in generating mode-locked pulses.
The evolution of the output pulse optical spectra at various pumping
4. Results & discussion powers is given in Fig. 6. As can be seen the patterns and shapes of the
spectra are almost identical, but the spectral bandwidth, Δ λ becomes
In order to generate the mode-locked pulses, the PC is adjusted slightly broader from 7.6 nm to 8.0 nm as the pump power is increased
accordingly, upon the insertion of SA. Mode-locked pulses are achieved from 130.20 mW to 280.50 mW. This is attributed to the spectral
at the threshold pump power of 100.80 mW. It should be noted that no bandwidth broadening with rising pump power as a result of the in-
mode-locked pulses are observed if the SA is not present in the cavity, creasing nonlinearity within the cavity [48]. This shows the de-
despite the pump and PC being tuned to its maximum range. This in- pendency of the spectral bandwidth on the pump power which is an-
dicates that the rGO-TiO2 coated SA is the sole component for gen- other typical feature of the dissipative soliton [49].
erating stable mode-locking operation in the laser cavity. The typical Fig. 7(a) displays the stability test of the passively mode-locked EDF
output characteristic of the mode-locked laser at a pump power of laser over an observation period of 60 min at a constant pump power of
268.1 mW is given in Fig. 5. Fig. 5(a) shows the optical spectrum of the 268.10 mW. The spectra are recorded using the RFSA at a lasing wa-
mode-locked pulses with a central wavelength of 1560.45 nm and 3-dB velength of 1560.45 nm. It can be seen that the spectrum remains
bandwidth of 2.47 nm. From the figure, three pairs of Kelly sidebands reasonably stable with no observable drifting in the central frequency
are distinctly observed in the spectrum, a typical characteristic of so- throughout the measurement period. The percentage of power fluc-
liton pulses in the lasers. The generation of Kelly sidebands are a result tuation is calculated to be less than 3.0%, suggesting that the mode-

99
H. Ahmad, et al.
locked pulses demonstrate high stability during the operation. Fur-
thermore, the low deviation of the SNR values in the range of
62.66–64.55 dB within the 60 min observation period validates the
stability of the proposed fiber laser’s output. This is given in Fig. 7(b).
Fig. 8 gives the variation of the pulse energy and output power with
respect to the pump power of the fiber laser. It can be seen that the
pulse energy and output power increases linearly against the pump
power, indicating the linear dependence of the pulse energy as well as
the output power on the pump power. The maximum average output
power is measured to be 1.51 mW which corresponds to the pulse en-
ergy of 134.98 pJ.
It is worth noticing that no damage is observed on the rGO-TiO2
coated D-shape fiber SA both physically and in terms of its perfor-
mance, even after the maximum pump power is reached. This indicates
that the fabricated SA possesses a damage threshold that is higher than
the maximum pump power available in this cavity. Previous work by
Sobon et. al. [50] reported that rGO on fused silica substrate results a
mode-locked pulses with a pulse energy of 29.8 pJ, lower than the re-
ported pulse energy in this work which is 139.4 pJ.
From Table 5, it can be seen that this work has a comparable center
of wavelength in generating mode-locked laser based on combining SA
and D-shape fiber with other works. This work also reports the second
lowest pulse duration as compared to Steinberg et. al. [53], though in
that work a lower maximum pulse energy than that reported here is
obtained. Song et. al. [26] reported a mode-locked laser with the
highest maximum pulse energy, but this work generates pulses with
lower pulse duration and higher repetition rate. Duan et. al. [51]
generated a mode-locked laser with a similar system using MoS2 as an
SA having a narrower repetition rate and wider pulse duration as
compared to other works in the above table. This shows that a different
performance of a mode-locked laser could be obtain by using different
SAs on a D-shape fiber as passive optical device in the fiber laser
system. Overall, mode-locked output with a smaller pulse duration and
higher pulse energy are preferred in photonics applications [54,55].
Additionally, it can be seen that the proposed laser operates in the
1560 nm region, also commonly known as the L-band region, which has
significant potential for the expansion of the current communications
bandwidth [56,57]. Furthermore, the all fiber nature of the cavity al-
lows for a tunable mechanism to be integrated into the design of the
laser, allowing for course or fine wavelength tuning [58]. Therefore, the
proposed work has a significant potential in generating passive mode-
locked laser particularly by combining D-shaped fiber with rGO-TiO2
nanohybrid, which leads to a multiple photonics application.
5. Conclusion
A new SA material composed of rGO nanosheets and TiO2 nano-
particles is proposed and developed for the generation of passively
mode-locking pulses at the wavelength of 1560.45 nm. Soliton-like
mode-locking pulses operating in the anomalous dispersion cavities are
successful generated, evidenced by the presence of Kelly sidebands in
the output optical spectrum. The laser generates pulses with a repeti-
tion rate of 11.19 MHz and pulse duration of 1.05 ps. A pulse energy of
134.98 pJ corresponds to the average output power of 1.51 mW are
achieved under the pump power of 280.5 mW. The obtained experi-
mental results have proven the potential of rGO-TiO2 nanohybrid as SA
in generating a highly stable mode-locking operation of the EDF laser
with the assistance of evanescent wave interaction. Owing the merits of
high stability and excellent damage threshold, the proposed SA could
be useful for high power pulse laser application.
Acknowledgement
We would like to thank the Ministry of Higher Education, Malaysia
for funding this research under the grant LRGS (2015)/NGOD/UM/KPT
and GA 010 – 2014 (ULUNG) and the University of Malaya for funding
100
Optics and Laser Technology 118 (2019) 93–101
this research under the grant RU 013 - 2018.
References
[1] Z. Zhang, C. Mou, Z. Yan, K. Zhou, L. Zhang, S. Turitsyn, Sub-100 fs mode-locked
erbium-doped fiber laser using a 45-tilted fiber grating, Opt. Exp. 21 (23) (2013)
28297–28303.
[2] S. Yan, J. Zhang, J. Zhou, W. Zhao, Characteristics of active mode-locked fiber ring
laser based on semiconductor optical amplifier, International Society for Optics and
Photonics, Passive Components and Fiber-based Devices V, 2008, p. 71342X.
[3] J. Černohorská, M. Písařík, P. Peterka, J. Aubrecht, R. Amani, O. Novák, M. Smrž,
M. Jelínek, A. Lucianetti, A. Endo, T. Mocek, High-energy subpicosecond 2-um fiber
laser, SPIE, SPIE Photonics Europe, 2018, p. 6.
[4] U. Keller, Recent developments in compact ultrafast lasers, Nature 424 (6950)
(2003) 831–838.
[5] S. Yamashita, Y. Inoue, S. Maruyama, Y. Murakami, H. Yaguchi, M. Jablonski,
S. Set, Saturable absorbers incorporating carbon nanotubes directly synthesized
onto substrates and fibers and their application to mode-locked fiber lasers, Opt.
Lett. 29 (14) (2004) 1581–1583.
[6] Y.-X. Guo, X.-H. Li, P.-L. Guo, H.-R. Zheng, Supercontinuum generation in an Er-
doped figure-eight passively mode-locked fiber laser, Opt. Exp. 26 (8) (2018)
9893–9900.
[7] E. Ding, W.H. Renninger, F.W. Wise, P. Grelu, E. Shlizerman, J.N. Kutz, High-energy
passive mode-locking of fiber lasers, Int. J. Opt. 2012 (2012) 17.
[8] K.Y. Lau, F.D. Muhammad, A.A. Latif, M.H. Abu Bakar, Z. Yusoff, M.A. Mahdi,
Passively mode-locked soliton femtosecond pulses employing graphene saturable
absorber, Opt. Laser Technol. 94 (2017) 221–227.
[9] X. Xu, J. Zhai, L. Li, Y. Chen, Y. Yu, M. Zhang, S. Ruan, Z. Tang, Passively mode-
locking erbium-doped fiber lasers with 0.3 nm single-walled carbon nanotubes, Sci.
Rep. 4 (2014) 6761.
[10] S.Y. Set, H. Yaguchi, Y. Tanaka, M. Jablonski, Laser mode locking using a saturable
absorber incorporating carbon nanotubes, J. Lightwave Technol. 22 (1) (2004)
51–56.
[11] D. Steinberg, H.G. Rosa, E.A.T.d. Souza, Influence of carbon nanotubes saturable
absorbers diameter on mode-locking erbium-doped fiber laser performance, J.
Lightwave Technol. 35 (21) (2017) 4804–4808.
[12] M. Pawliszewska, T. Martynkien, A. Przewłoka, J. Sotor, Dispersion-managed Ho-
doped fiber laser mode-locked with a graphene saturable absorber, Opt. Lett. 43 (1)
(2018) 38–41.
[13] H. Zhang, D. Tang, L. Zhao, Q. Bao, K. Loh, Large energy mode locking of an er-
bium-doped fiber laser with atomic layer graphene, Opt. Exp. 17 (20) (2009)
17630–17635.
[14] Z. Sun, T. Hasan, F. Torrisi, D. Popa, G. Privitera, F. Wang, F. Bonaccorso,
D.M. Basko, A.C. Ferrari, Graphene mode-locked ultrafast laser, ACS Nano 4 (2)
(2010) 803–810.
[15] Y. Hu, X. Jin, G. Hu, M. Zhang, Q. Wu, Z. Zheng, T. Hasan, Hybrid mode-locked
erbium-doped fiber laser with black phosphorus saturable absorber, Conference on
Lasers and Electro-Optics, Optical Society of America, San Jose, California, 2018, p.
SF3I.4.
[16] M. Pawliszewska, Y. Ge, Z. Li, H. Zhang, J. Sotor, Fundamental and harmonic mode-
locking at 2.1 μm with black phosphorus saturable absorber, Opt. Exp. 25 (15)
(2017) 16916–16921.
[17] N.A.A. Kadir, E.I. Ismail, A.A. Latiff, H. Ahmad, H. Arof, S.W. Harun, Transition
metal dichalcogenides (WS2 and MoS2) saturable absorbers for mode-locked er-
bium-doped fiber lasers, Chin. Phys. Lett. 34 (1) (2017) 014202.
[18] D. Mao, X. Cui, X. Gan, M. Li, W. Zhang, H. Lu, J. Zhao, Passively Q-switched and
mode-locked fiber laser based on an ReS2 saturable absorber, IEEE J. Sel. Top.
Quant. Electron. 24 (3) (2018) 1–6.
[19] J. Du, Q. Wang, G. Jiang, C. Xu, C. Zhao, Y. Xiang, Y. Chen, S. Wen, H. Zhang,
Ytterbium-doped fiber laser passively mode locked by few-layer molybdenum dis-
ulfide (MoS2) saturable absorber functioned with evanescent field interaction, Sci.
Rep. 4 (2014) 6346.
[20] D. Mao, X. She, B. Du, D. Yang, W. Zhang, K. Song, X. Cui, B. Jiang, T. Peng, J. Zhao,
Erbium-doped fiber laser passively mode locked with few-layer WSe2/MoSe2 na-
nosheets, Sci. Rep. 6 (2016) 23583.
[21] Y.I. Jhon, J. Lee, Y.M. Jhon, J.H. Lee, Topological insulators for mode-locking of 2-
μm fiber lasers, IEEE J. Sel. Top. Quant. Electron. 24 (5) (2018) 1–8.
[22] P. Yan, R. Lin, S. Ruan, A. Liu, H. Chen, Y. Zheng, S. Chen, C. Guo, J. Hu, A practical
topological insulator saturable absorber for mode-locked fiber laser, Sci. Rep. 5
(2015) 8690.
[23] J. Bogusławski, G. Soboń, R. Zybała, K. Mars, A. Mikuła, K.M. Abramski, J. Sotor,
Investigation on pulse shaping in fiber laser hybrid mode-locked by Sb2 Te3 sa-
turable absorber, Opt. Exp. 23 (22) (2015) 29014–29023.
[24] Z. Luo, D. Wu, B. Xu, H. Xu, Z. Cai, J. Peng, J. Weng, S. Xu, C. Zhu, F. Wang, Two-
dimensional material-based saturable absorbers: towards compact visible-wave-
length all-fiber pulsed lasers, Nanoscale 8 (2) (2016) 1066–1072.
[25] Y. Zhang, J. Zhu, P. Li, X. Wang, H. Yu, K. Xiao, C. Li, G. Zhang, All-fiber Yb-doped
fiber laser passively mode-locking by monolayer MoS2 saturable absorber, Opt.
Commun. 413 (2018) 236–241.
[26] Y.-W. Song, S.-Y. Jang, W.-S. Han, M.-K. Bae, Graphene mode-lockers for fiber lasers
functioned with evanescent field interaction, Appl. Phys. Lett. 96 (5) (2010)
051122.
[27] V. Ashith, G.K. Rao, R. Smitha, S.N. Moger, Study of micro-structural, optical and
electrical properties of TiO2 films obtained from micro-controller based SILAR
method, Ceram. Int. 44 (15) (2018) 17623–17629.
H. Ahmad, et al.
[28] M. Jung, J. Koo, P. Debnath, Y.-W. Song, J.H. Lee, A mode-locked 1.91 µm fiber
laser based on interaction between graphene oxide and evanescent field, Appl.
Phys. Exp. 5 (11) (2012) 112702.
[29] R. Nirmala, J.W. Jeong, R. Navamathavan, H.Y. Kim, Synthesis and electrical
properties of TiO2 nanoparticles embedded in polyamide-6 nanofibers via electro-
spinning, Nano-Micro Lett. 3 (1) (2011) 56–61.
[30] G. Liu, L. Wang, B. Wang, T. Gao, D. Wang, A reduced graphene oxide modified
metallic cobalt composite with superior electrochemical performance for super-
capacitors, RSC Adv. 5 (78) (2015) 63553–63560.
[31] N. Yusoff, P. Rameshkumar, M.M. Shahid, S.-T. Huang, N.M. Huang, Amperometric
detection of nitric oxide using a glassy carbon electrode modified with gold nano-
particles incorporated into a nanohybrid composed of reduced graphene oxide and
Nafion, Microchimica Acta 184 (9) (2017) 3291–3299.
[32] M.K. Rabchinskii, V.V. Shnitov, A.T. Dideikin, A.E. Aleksenskii, S.P. Vul’,
M.V. Baidakova, I.I. Pronin, D.A. Kirilenko, P.N. Brunkov, J. Weise, Nanoscale
perforation of graphene oxide during photoreduction process in the argon atmo-
sphere, J. Phys. Chem. C 120 (49) (2016) 28261–28269.
[33] W. Wang, Y. Liu, J. Qu, Y. Chen, Z. Shao, Nitrogen-doped TiO 2 microspheres with
hierarchical micro/nanostructures and rich dual-phase junctions for enhanced
photocatalytic activity, RSC Adv. 6 (47) (2016) 40923–40931.
[34] N. Yusoff, A. Pandikumar, A. Marlinda, N. Huang, H. Lim, Nanosized graphene/
Nafion hybrid modified electrode for electrochemical detection of dopamine, Sci.
Adv. Mater. 7 (12) (2015) 2692–2703.
[35] W. Wang, Z. Wang, J. Liu, Z. Luo, S.L. Suib, P. He, G. Ding, Z. Zhang, L. Sun, Single-
step one-pot synthesis of TiO2 nanosheets doped with sulfur on reduced graphene
oxide with enhanced photocatalytic activity, Sci. Rep. 7 (2017) 46610.
[36] N. Yusoff, P. Rameshkumar, N.M. Huang, Amperometric determination of L-cy-
steine using a glassy carbon electrode modified with palladium nanoparticles grown
on reduced graphene oxide in a Nafion matrix, Microchimica Acta 185 (4) (2018)
246.
[37] N. Li, X. Zhang, W. Zhou, Z. Liu, G. Xie, Y. Wang, Y. Du, High quality sulfur-doped
titanium dioxide nanocatalysts with visible light photocatalytic activity from non-
hydrolytic thermolysis synthesis, Inorg. Chem. Front. 1 (7) (2014) 521–525.
[38] K. Tey, M. Rahman, A. Rosol, M. Rusdi, M. Mahyuddin, S. Harun, A. Latiff, Q-
switched double-clad Ytterbium-doped fiber laser using MoS2 flakes saturable ab-
sorber, IOP conference series: materials science and engineering, IOP Publishing,
2017, p. 012054.
[39] J. Jeon, J. Lee, J.H. Lee, Numerical study on the minimum modulation depth of a
saturable absorber for stable fiber laser mode locking, JOSA B 32 (1) (2015) 31–37.
[40] H. Hu, X. Zhang, W. Li, N.K. Dutta, Hybrid mode-locked fiber ring laser using
graphene and charcoal nanoparticles as saturable absorbers, Micro-and
Nanotechnology Sensors, Systems, and Applications VIII, International Society for
Optics and Photonics, 2016, p. 983630.
[41] R. Woodward, E. Kelleher, R. Howe, G. Hu, F. Torrisi, T. Hasan, S. Popov, J. Taylor,
Tunable Q-switched fiber laser based on saturable edge-state absorption in few-
layer molybdenum disulfide (MoS 2), Opt. Express 22 (25) (2014) 31113–31122.
[42] M. Jung, J. Koo, J. Park, Y.-W. Song, Y.M. Jhon, K. Lee, S. Lee, J.H. Lee, Mode-
locked pulse generation from an all-fiberized, Tm-Ho-codoped fiber laser in-
corporating a graphene oxide-deposited side-polished fiber, Opt. Exp. 21 (17)
101
Optics and Laser Technology 118 (2019) 93–101
(2013) 20062–20072.
[43] K. Lau, E. Ng, M.A. Bakar, A. Abas, M. Alresheedi, Z. Yusoff, M. Mahdi, Low
threshold linear cavity mode-locked fiber laser using microfiber-based carbon na-
notube saturable absorber, Opt. Laser Technol. 102 (2018) 240–246.
[44] Y. Li, L. Gao, W. Huang, C. Gao, M. Liu, T. Zhu, All-fiber mode-locked laser via short
single-wall carbon nanotubes interacting with evanescent wave in photonic crystal
fiber, Opt. Exp. 24 (20) (2016) 23450–23458.
[45] H. Ahmad, M. Samion, N. Yusoff, Soliton mode-locked thulium-doped fiber laser
with cobalt oxide saturable absorber, Opt. Fiber Technol. 45 (2018) 122–127.
[46] T. Noronen, S. Firstov, E. Dianov, O.G. Okhotnikov, 1700 nm dispersion managed
mode-locked bismuth fiber laser, Sci. Rep. 6 (2016) 24876.
[47] M. Yue, J. Si, L. Yan, Y. Yu, X. Hou, Enhanced nonlinear optical properties of re-
duced graphene oxide decorated with silver nanoparticles, Opt. Mater. Exp. 8 (3)
(2018) 698–703.
[48] J. Ma, J. Wang, D. Shen, H. Yu, H. Zhang, D. Tang, Dissipative soliton operation of a
diode pumped Yb: NaY(WO4)2 laser, Opt. Exp. 23 (25) (2015) 32311–32317.
[49] Q. Wang, Y. Chen, L. Miao, G. Jiang, S. Chen, J. Liu, X. Fu, C. Zhao, H. Zhang, Wide
spectral and wavelength-tunable dissipative soliton fiber laser with topological
insulator nano-sheets self-assembly films sandwiched by PMMA polymer, Opt. Exp.
23 (6) (2015) 7681–7693.
[50] G. Sobon, J. Sotor, J. Jagiello, R. Kozinski, M. Zdrojek, M. Holdynski, P. Paletko,
J. Boguslawski, L. Lipinska, K.M. Abramski, Graphene oxide vs. reduced graphene
oxide as saturable absorbers for Er-doped passively mode-locked fiber laser, Opt.
Exp. 20 (17) (2012) 19463–19473.
[51] L.-N. Duan, Y.-L. Su, Y.-G. Wang, L. Li, X. Wang, Y.-S. Wang, Passively mode-locked
erbium-doped fiber laser via a D-shape-fiber-based MoS2 saturable absorber with a
very low nonsaturable loss, Chin. Phys. B 25 (2) (2016) 024206.
[52] H.B. Ahmad, S. Soltani, K. Thambiratnam, M. Yasin, Highly stable mode-locked
fiber laser with graphene oxide-coated side-polished D-shaped fiber saturable ab-
sorber, SPIE (2018) 9.
[53] D. Steinberg, J.D. Zapata, E.A.T. de Souza, L.A. Saito, Mechanically exfoliated
graphite onto D-shaped optical fiber for femtosecond mode-locked erbium-doped
fiber laser, J. Lightwave Technol. 36 (10) (2018) 1868–1874.
[54] M.K. Dasa, C. Markos, M. Maria, C.R. Petersen, P.M. Moselund, O. Bang, High-pulse
energy supercontinuum laser for high-resolution spectroscopic photoacoustic ima-
ging of lipids in the 1650–1850 nm region, Biomed. Opt. Exp. 9 (4) (2018)
1762–1770.
[55] R. Mary, D. Choudhury, A.K. Kar, Applications of fiber lasers for the development of
compact photonic devices, IEEE J. Sel. Top. Quantum Electron. 20 (5) (2014)
72–84.
[56] S. Harun, N. Tamchek, P. Poopalan, H. Ahmad, Double-pass L-band EDFA with
enhanced noise figure characteristics, IEEE Photonics Technol. Lett. 15 (8) (2003)
1055–1057.
[57] S. Harun, S. Low, P. Poopalan, H. Ahmad, Gain clamping in L-band erbium-doped
fiber amplifier using a fiber Bragg grating, IEEE Photonics Technol. Lett. 14 (3)
(2002) 293–295.
[58] H. Ahmad, M. Zulkifli, A. Latif, S. Harun, Tunable dual wavelength fiber laser in-
corporating AWG and optical channel selector by controlling the cavity loss, Opt.
Commun. 282 (24) (2009) 4771–4775.